N-doped CoAl oxides from hydrotalcites with enhanced oxygen vacancies for excellent low-temperature propane oxidation

• Published in: Journal of environmental sciences (China) 2022-06, Vol.116, p.79-89
• Main Authors: Wu, Enhui, Lin, Daifeng, Chen, Yinye, Feng, Xiaoshan, Niu, Kui, Luo, Yongjin, Huang, Baoquan, Qiu, Jianbin, Qian, Qingrong, Chen, Qinghua
• Format: Article
• Language: English
• Subjects: Aluminum Hydroxide; Co species; Coal; Hydrotalcite derived oxides; Magnesium Hydroxide; N doping; Oxides - chemistry; Oxygen - analysis; Oxygen vacancies; Propane; Propane oxidation; Temperature
• ISSN: 1001-0742; 1878-7320
• DOI: 10.1016/j.jes.2021.07.003

A series of nitrogen-doped CoAlO (N-CoAlO) were constructed by a hydrothermal route combined with a controllable NH3 treatment strategy. The effects of NH3 treatment on the physico-chemical properties and oxidation activities of N-CoAlO catalysts were investigated. In comparison to CoAlO, a smallest content decrease in surface Co3+ (serving as active sites) while a largest increased amount of surface Co2+ (contributing to oxygen species) are obtained over N-CoAlO/4h among the N-CoAlO catalysts. Meanwhile, a maximum N doping is found over N-CoAlO/4h. As a result, N-CoAlO/4h (under NH3 treatment at 400°C for 4 hr) with rich oxygen vacancies shows optimal catalytic activity, with a T90 (the temperature required to reach a 90% conversion of propane) at 266°C. The more oxygen vacancies are caused by the co-operative effects of N doping and suitable reduction of Co3+ for N-CoAlO/4h, leading to an enhanced oxygen mobility, which in turn promotes C3H8 total oxidation activity dominated by Langmuir-Hinshelwood mechanism. Moreover, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) analysis shows that N doping facilities the decomposition of intermediate species (propylene and formate) into CO2 over the catalyst surface of N-CoAlO/4h more easily. Our reported design in this work will provide a promising way to develop abundant oxygen vacancies of Co-based catalysts derived from hydrotalcites by a simple NH3 treatment. [Display omitted]